表面活性剂辅助农药在锂皂石中的插层及其性能

doi:10.11901/1005.3093.2020.215

材料研究学报

2021, Vol. 35

Issue (2): 81-92 DOI: 10.11901/1005.3093.2020.215

研究论文

本期目录 | 过刊浏览

表面活性剂辅助农药在锂皂石中的插层及其性能

刘洁翔¹(

), 刘蕊¹, 张晓光²(

)

^1.河北工业大学化工学院天津 300130
^2.南开大学化学学院天津 300071

Preparation and Property of Laponite with Pesticide Intercalation

LIU Jiexiang¹(

), LIU Rui¹, ZHANG Xiaoguang²(

)

^1.School of Chemical Engineering, Hebei University of Technology, Tianjin 300130, China
^2.College of Chemistry, Nankai University, Tianjin 300071, China

引用本文:

刘洁翔, 刘蕊, 张晓光. 表面活性剂辅助农药在锂皂石中的插层及其性能[J]. 材料研究学报, 2021, 35(2): 81-92.
Jiexiang LIU, Rui LIU, Xiaoguang ZHANG. Preparation and Property of Laponite with Pesticide Intercalation[J]. Chinese Journal of Materials Research, 2021, 35(2): 81-92.

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摘要:

利用两性表面活性剂十六烷基磺基甜菜碱(SB)的辅助作用实现了农药功夫菊酯(LCT)在锂皂石(LAP)中的插层。先用离子交换法将SB、十二烷基羧基甜菜碱(DCB)、十二烷基氧化胺(OA)和阳离子表面活性剂十六烷基三甲基溴化铵(CTAB)分别插层LAP，然后用SB胶束将LCT引入层间，得到LCT/SB-LAP、LCT/DCB-SB-LAP、LCT/OA-SB-LAP和LCT/CTAB-SB-LAP复合材料。采用X射线衍射(XRD)、液体核磁共振(¹HNMR)、电感耦合等离子发射光谱(ICP-OES)、傅里叶变换红外光谱(FT-IR)、热重/差热分析(TGA/DTA)和扫描电镜(SEM)对复合材料进行了表征。结果表明，LCT/SB-LAP、LCT/DCB-SB-LAP、LCT/OA-SB-LAP和LCT/CTAB-SB-LAP的层间高度分别为3.61、3.13、3.13和3.41 nm；LCT伴随SB分子成功进入LAP层间。提出了LCT在LAP中的插层机理。对复合材料中LCT释放行为的研究结果表明，释放速率和累积释放量主要依赖表面活性剂类型及其在层间的排列方式。

关键词 ：复合材料, 锂皂石杂化材料, 胶束, 功夫菊酯, 释放行为

Abstract：

The laponite (LAP) with intercalation of pesticide lambda-cyhalothrin (LCT) was prepared with surfactant of 3-sulphonyl hexadecyldimethylamine (SB) as accessory ingredient. The zwitterionic surfactant of SB, dodecyl dimethyl carboxylbetaine (DCB), N,N-dimethyldodecylamine N-oxide(OA) and cationic surfactant cetyl trimethyl ammonium bromide (CTAB) were separately intercalated into laponite (LAP), and then LCT was solubilized into SB micelles and intercalated into the galleries finally composites of LCT/SB-LAP, LCT/DCB-SB-LAP, LCT/OA-SB-LAP and LCT/CTAB-SB-LAP were obtained. These composites were systematically characterized by powder X-ray diffraction (XRD), liquid state nuclear magnetic resonance (¹H NMR), inductively coupled plasma-optical emission spectroscopy (ICP-OES), fourier transform infrared (FT-IR) spectroscopy, thermogravimetry/differential thermal analysis (TGA/DTA) and scanning electron microscope (SEM). The results show that the interlamellar spacings of LCT/SB-LAP, LCT/DCB-SB-LAP, LCT/OA-SB-LAP and LCT/CTAB-SB-LAP were 3.61, 3.13, 3.13 and 3.41 nm, respectively. The LCT companying SB molecules entered into the interlamellar of LAP was confirmed by ¹H NMR, ICP-OES and spectroscopy FT-IR. The intercalation mechanism of LCT induced by SB micelles was proposed. The release behavior of LCT from composites was investigated and analyzed. The release rates and cumulative amounts are mainly dependent on type and arrangement of surfactants in the interlamellar spacing.

Key words： composite laponite hybrid material micelle lambda-cyhalothrin release behavior

收稿日期: 2020-06-08

ZTFLH:

O641

基金资助:国家重点研发计划(2016YFD0200707)

作者简介: 刘洁翔，女，1973年生，博士

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https://www.cjmr.org/CN/10.11901/1005.3093.2020.215 或 https://www.cjmr.org/CN/Y2021/V35/I2/81

图1 SB、DCB、OA和CTAB的结构示意图

图2 SB(OA、DCB、CTAB)-LAP，LCT/SB-LAP 和 LCT/DCB(OA、CTAB)-SB-LAP的XRD谱

图3 表面活性剂和LCT分子在LAP层间排列的示意图

图4 LCT/DCB-SB-LAP、LCT/OA-SB-LAP和LCT/CTAB-SB-LAP的1H NMR谱图

表1 不同样品的S含量(质量分数)

图5 样品的红外谱图

图6 样品的TGA/DTA曲线

图7 样品的SEM照片

图8 LCT/SB-LAP、LCT/DCB-SB-LAP、LCT/OA-SB-LAP和LCT/CTAB-SB-LAP在不同缓冲溶液中的释放曲线

图9 LCT/SB-LAP、LCT/DCB-SB-LAP、LCT/OA-SB-LAP和LCT/CTAB-SB-LAP的准二级动力学拟合曲线

图10 LCT/SB-LAP、LCT/DCB-SB-LAP、LCT/OA-SB-LAP和LCT/CTAB-SB-LAP的抛物线扩散拟合曲线

表2 不同复合材料的Zeta电势

表3 由准二级动力学和抛物线扩散模型拟合释放的数据

1	Pieper H, Bosbach D, Panak P J, et al. Eu(III) coprecipitation with the trioctahedral clay mineral, hectorite [J]. Clays Clay Miner., 2006, 54: 45
2	Baskaralingam P, Pulikesi M, Ramamurthi V, et al. Modified hectorites and adsorption studies of a reactive dye [J]. Appl. Clay Sci., 2007, 37: 207
3	Lair V, Carbonnell C, Peyre V, et al. Potentiometric determination of adsorption isotherms of dodecyldimethylamine-N-oxide onto laponite [J]. Colloids Surf. A, 2003, 212: 265
4	Lamont R E, Ducker W A. Surface-induced transformations for surfactant aggregates [J]. J. Am. Chem. Soc., 1998, 120: 7602
5	Thiebault T, Brendlé J, Augé G, et al. Zwitterionic-surfactant modified LAPONITE®s for removal of ions (Cs⁺, Sr²⁺ and Co²⁺) from aqueous solutions as a sustainable recovery method for radionuclides from aqueous wastes [J]. Green Chem., 2019, 21: 5118
6	Esumi K, Yoshida K, Torigoe K, et al. Sorption of 2-naphthol and copper ions by cationic surfactant-adsorbed laponite [J]. Colloids Surf. A, 1999, 160: 247
7	Nair B P, Sindhu M, Nair P D. Polycaprolactone-laponite composite scaffold releasing strontium ranelate for bone tissue engineering applications [J]. Colloids Surf. B, 2016, 143: 423
8	Pacelli S, Paolicelli P, Moretti G, et al. Gellan gum methacrylate and laponite as an innovative nanocomposite hydrogel for biomedical applications [J]. Eur. Polym. J., 2016, 77: 114
9	Roozbahani M, Kharaziha M, Emadi R. pH sensitive dexamethasone encapsulated laponite nanoplatelets: release mechanism and cytotoxicity [J]. Int. J. Pharm., 2017, 518: 312
10	Wang S G, Wu Y L, Guo R, et al. Laponite nanodisks as an efficient platform for doxorubicin delivery to cancer cells [J]. Langmuir, 2013, 29: 5030
11	Wang G Y, Maciel D, Wu Y L, et al. Amphiphilic polymer-mediated formation of laponite-based nanohybrids with robust stability and pH sensitivity for anticancer drug delivery [J]. ACS Appl. Mater. Interfaces, 2014, 6: 16687
12	Wu Y L, Guo R, Wen S H, et al. Folic acid-modified laponite nanodisks for targeted anticancer drug delivery [J]. J. Mater. Chem. B, 2014, 2: 7410
13	Chen G X, Li D, Li J C, et al. Targeted doxorubicin delivery to hepatocarcinoma cells by lactobionic acid-modified laponite nano-disks [J]. New J. Chem., 2015, 39: 2847
14	Xiao S L, Castro R, Maciel D, et al. Fine tuning of the pH-sensitivity of laponite-doxorubicin nanohybrids by polyelectrolyte multilayer coating [J]. Mater. Sci. Eng. C, 2016, 60: 348
15	Hamilton A R, Roberts M, Hutcheon G A, et al. Formulation and antibacterial properties of clay mineral-tetracycline and-doxycycline composites [J]. Appl. Clay Sci., 2019, 179: 105148
16	Liu J X, Zhang X G, Zhang Y Q. Preparation and release behavior of chlorpyrifos adsolubilized into layered zinc hydroxide nitrate intercalated with dodecylbenzenesulfonate [J]. ACS Appl. Mater. Interfaces, 2015, 7: 11180
17	Zhang H, Pan D K, Zou K, et al. A novel core-shell structured magnetic organic-inorganic nanohybrid involving drug-intercalated layered double hydroxides coated on a magnesium ferrite core for magnetically controlled drug release [J]. J. Mater. Chem., 2009, 19: 3069
18	Jiang W, Su H J, Huo H Y, et al. Synthesis and properties of surface molecular imprinting adsorbent for removal of Pb²⁺ [J]. Appl. Biochem. Biotechnol., 2010, 160: 467
19	Lu L F, Gao M L, Yang S F, et al. Preparation and adsorption for ciprofloxacin of bentonite modified by zwitterionic surfactant [J]. Chin. J. Mater. Res., 2013, 27: 576
19	路来福, 高芒来, 杨森锋等. 两性表面活性剂改性膨润土的制备及其对环丙沙星的吸附性能 [J]. 材料研究学报, 2013, 27: 576
20	Jung H, Kim H M, Choy Y B, et al. Laponite-based nanohybrid for enhanced solubility and controlled release of itraconazole [J]. Int. J. Pharm., 2008, 349: 283
21	Wang J X, Morales-Collazo O, Wei A. Micellization and single-particle encapsulation with dimethylammoniopropyl sulfobetaines [J]. ACS Omega, 2017, 2: 1287
22	Liu J X, Wang J L, Zhang X G, et al. Preparation and structural characterization of zwitterionic surfactant intercalated into NiZn-layered hydroxide salts [J]. J. Phys. Chem. Solids, 2015, 85: 180
23	Maeda H. A thermodynamic analysis of the hydrogen ion titration of micelles [J]. J. Colloid Interface Sci., 2003, 263: 277
24	Fan N Q, Fan Y X, Tong D S, et al. Study on structure characteristics of organic hectorite hydrothermally synthesized in reaction medium with the presence of surfactants [J]. J. Chem. Eng. Chin. Univ., 2010, 24: 852
24	范能全, 范永仙, 童东绅等. 表面活性剂介质中有机化锂皂石的水热合成及结构特征 [J]. 高校化学工程学报, 2010, 24: 852
25	Liu J X, Wang J L, Zhang X G. Intercalation, characterization and release behavior of imidacloprid into layered hydroxide salts by coupling of (3-glycidyloxypropyl) trimethoxysilane [J]. Colloids Surf., 2018, 553A: 42
26	Li T, Liu Z L, Xiao M, et al. In vitro and in vivo studies of a gelatin/carboxymethyl chitosan/LAPONITE® composite scaffold for bone tissue engineering [J]. RSC Adv., 2017, 7: 54100
27	Tang L C, Wei W, Wang X H, et al. Laponite® nanorods regulating degradability, acidic-alkaline microenvironment, apatite mineralization and MC3T3-E1 cells responses to poly(butylene succinate) based bio-nanocomposite scaffolds [J]. RSC Adv., 2018, 8: 10794
28	Kuźniarska-Biernacka I, Silva A R, Carvalho A P, et al. Organo-laponites as novel mesoporous supports for manganese(III) salen catalysts [J]. Langmuir, 2005, 21: 10825
29	Zhang P, Wang J, Jia Y, et al. Encapsulating spinel nancrystals in Laponite cages and applications in molecular oxidation of cyclohexane [J]. Appl. Clay Sci., 2019, 181: 105226
30	Zhang L, Li J J, Liu T Q. Preparation and properties of water-based cypermethrin microemulsion [J]. J. Yangzhou Univ. (Nat. Sci. Ed.), 2012, 15(2): 38
30	张龙, 李佳佳, 刘天晴. 水基型氯氰菊酯农药微乳剂的研制与性质 [J]. 扬州大学学报(自然科学版), 2012, 15(2): 38
31	Bi G, Feng Z G, Tian S Z, et al. Infrared spectroscopy study on the photolysis products of pyrthroids [J]. Chin. J. Spectrosc. Lab., 1995, 12(6): 39
31	毕刚, 冯子刚, 田世忠等. 拟除虫菊酯光解产物的红外图谱研究 [J]. 光谱实验室, 1995, 12(6): 39
32	Ma L Y, Chen Q Z, Zhu J X, et al. Adsorption of phenol and Cu(II) onto cationic and zwitterionic surfactant modified montmorillonite in single and binary systems [J]. Chem. Eng. J., 2016, 283: 880
33	Zhou C H, Du Z X, Li X N, et al. Structure development of hectorite in hydrothermal crystallization synthesis process [J]. Chinese J. Inorg. Chem., 2005, 21: 1327
33	周春晖, 杜泽学, 李小年等. 水热体系合成锂皂石结构的演化和影响规律研究 [J]. 无机化学学报, 2005, 21: 1327
34	Wang B X, Zhou M, Rozynek Z, et al. Electrorheological properties of organically modified nanolayered laponite: influence of intercalation, adsorption and wettability [J]. J. Mater. Chem., 2009, 19: 1816
35	Li J Y, Yang Y, Yu Y B, et al. LAPONITE® nanoplatform functionalized with histidine modified oligomeric hyaluronic acid as an effective vehicle for the anticancer drug methotrexate [J]. J. Mater. Chem. B, 2018, 6: 5011
36	Jatav S, Joshi Y M. Chemical stability of laponite in aqueous media [J]. Appl. Clay Sci., 2014, 97-98: 72
37	Dening T J, Thomas N, Rao S S, et al. Montmorillonite and laponite clay materials for the solidification of lipid-based formulations for the basic drug blonanserin: In vitro and in vivo Investigations [J]. Mol. Pharm., 2018, 15: 4148
38	Sanchez-Martin M J, Rodriguez-Cruz M S, Andrades M S, et al. Efficiency of different clay minerals modified with a cationic surfactant in the adsorption of pesticides: Influence of clay type and pesticide hydrophobicity [J]. Appl. Clay Sci., 2006, 31: 216
39	McLauchlin A R, Thomas N L. Preparation and thermal characterisation of poly(lactic acid) nanocomposites prepared from organoclays based on an amphoteric surfactant [J]. Polym. Degrad. Stab., 2009, 94: 868

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